Data for M. Pizzochero, G. Borin Barin, K. Čerņevičs, S. Wang, P. Ruffieux, R. Fasel, O. V. Yazyev , J. Phys. Chem. Lett. 12, 4692−4696 (2021) DOI: 10.1021/acs.jpclett.1c00921 URL: https://pubs.acs.org/doi/10.1021/acs.jpclett.1c00921 The following zip file contains two folders corresponding to the experimental and theoretical data: 1)Experimental: -Raw files (in .txt) for the STM image and the three NC-AFM images in figure 1 for the paper 2)Theoretical: -Further split in two folder corresponding to the edge geometry - ZigZag or Armchair and containing: *Relaxations: Input and output data of relaxation of the atomic structure of AGNR hosting a single (1_Single-Defect) or double (2_Double-Defect) bite defects, this latter for each othe five configurations discussed in the manuscript (alpha, beta, ..., epsilon). *Transport: Input and output data of charge transport calculations across AGNR hosting a single (1_Single-Defect), double (2_Double-Defect), or no (3_Pristine-AC) bite defect. For the single- and no-bite defect case, the data to perform finite-bias calculations (I-V) curves are also given for different values of voltage. All numerical calculations were carried out by Siesta v4.1-b4.